Ultrasonic enhanced liquid-liquid interfacial reaction for improving the synthesis of Iron-doped carbon dots (Fe-CDs) for achieving superior photocatalytic performance.

The precise and controllable preparation of carbon nanomaterials under mild conditions poses a great challenge, especially for metal-catalysed multiphase preparation. This work proposes an efficient method that utilizing high-density ultrasound to enhance the liquid-liquid interfacial reaction system. Iron-doped carbon dots (Fe-CDs) are successfully synthesized in such a normal temperature and atmospheric-pressure reaction condition. It is shown that transient cavitation provides a high-temperature and high-pressure microenvironment for the preparation of Fe-CDs. Moreover, the size of the reactant droplets is reduced from 200.0 ± 17.3 µm to 8.1 ± 2.9 µm owing to the acoustic flow and cavitation effects, which increases the specific surface area of the two reacting phases and improves the mass transfer coefficient by more than 252.0 %. As a result, the yield increases by more than an order of magnitude (from 0.7 ± 0.1 % to 11.9 ± 0.2 %) and the Fe doping rate reaches 20.9 %. The photocatalytic oxidation conversion of 1,4-Dihydropyridine (1,4-DHP) using the obtained Fe-CDs is as high as 98.2 %. This research gives a new approach for the efficient and safe production of Fe-CDs, which is promising for industrial applications.

A comprehensive overview of graph neural network-based approaches to clustering for spatial transcriptomics.

Spatial transcriptomics technologies enable researchers to accurately quantify and localize messenger ribonucleic acid (mRNA) transcripts at a high resolution while preserving their spatial context. The identification of spatial domains, or the task of spatial clustering, plays a crucial role in investigating data on spatial transcriptomes. One promising approach for classifying spatial domains involves the use of graph neural networks (GNNs) by leveraging gene expressions, spatial locations, and histological images. This study provided a comprehensive overview of the most recent GNN-based methods of spatial clustering methods for the analysis of data on spatial transcriptomics. We extensively evaluated the performance of current methods on prevalent datasets of spatial transcriptomics by considering their accuracy of clustering, robustness, data stabilization, relevant requirements, computational efficiency, and memory use. To this end, we explored 60 clustering scenarios by extending the essential frameworks of spatial clustering for the selection of the GNNs, algorithms of downstream clustering, principal component analysis (PCA)-based reduction, and refined methods of correction. We comparatively analyzed the performance of the methods in terms of spatial clustering to identify their limitations and outline future directions of research in the field. Our survey yielded novel insights, and provided motivation for further investigating spatial transcriptomics.

The spatiotemporal dynamics of spatially variable genes in developing mouse brain revealed by a novel computational scheme.

To understand how brain regions form and work, it is important to explore the spatially variable genes (SVGs) enriched in specific brain regions during development. Spatial transcriptomics techniques provide opportunity to select SVGs in the high-throughput way. However, previous methods neglected the ranking order and combinatorial effect of SVGs, making them difficult to automatically select the high-priority SVGs from spatial transcriptomics data. Here, we proposed a novel computational pipeline, called SVGbit, to rank the individual and combinatorial SVGs for marker selection in various brain regions, which was tested in different kinds of public datasets for both human and mouse brains. We then generated the spatial transcriptomics and immunohistochemistry data from mouse brain at critical embryonic and neonatal stages. The results show that our ranking and clustering scheme captures the key SVGs which coincide with known anatomic regions in the developing mouse brain. More importantly, SVGbit can facilitate the identification of multiple gene combination sets in different brain regions. We identified three dynamical sub-regions which can be segregated by the staining of Sox2 and Calb2 in thalamus, and we also found that Nr4a2 expression gradually segregates the neocortex and hippocampus during the development. In summary, our work not only reveals the spatiotemporal dynamics of individual and combinatorial SVGs in developing mouse brain, but also provides a novel computational pipeline to facilitate the selection of marker genes from spatial transcriptomics data.

In Situ Solution-Processed Submicron Thick SiOx Cy /a-SiNx (O):H Composite Barrier Film for Polymer:Non-Fullerene Photovoltaics.

Aiming to improve the environmental stability of organic photovoltaics, a multilayered SiOx Cy /a-SiNx (O):H composite barrier film coated with a hydrophobic perfluoro copolymer stop layer for polymer:non-fullerene solar cells is developed. The composite film is prepared by spin-coating of polysilicone and perhydropolysilazane (PHPS) following a densification process by vacuum ultraviolet irradiation in an inert atmosphere. The transformation of polysilicone and PHPS to SiOx Cy and a-SiNx (O):H is confirmed by Fourier transform infrared and energy-dispersive X-ray spectroscopy measurement. However, the as-prepared PHPS-derived silicon nitride (PDSN) can react with moisture in the ambient atmosphere, yielding microscale defects and a consequent poor barrier performance. Treating the incomplete PDSN with methanol vapor significantly densifies the film yielding low water vapor transmission rates (WVTRs)of 5.0 × 10-1 and 2.0 × 10-1 g m-2  d-1 for the one- and three-couple of SiOx Cy /a-SiNx (O):H (CON) composite films, respectively. By incorporating a thin hydrophobic perfluoro copolymer layer, the three-coupled methanol-treated CON film with a total thickness of 600 nm shows an extremely low WVTR of 8.7 × 10-4 g m-2  d-1 . No performance decay is measured for the PM6:Y6 and PM6:L8-BO cells after such an encapsulation process. These encapsulated polymer cells show good stability storaged at 25 °C/50% relative humidity, or under simulated extreme rainstorm tests.

Ultrasonic enhancement of microdroplet-based interfacial reaction for improving the synthesis of Ag2S QDs.

Ag2S quantum dots (QDs) have aroused extensive concerns in intravital imaging field due to their merits of narrow bandgap, low biological toxicity and decent fluorescence emission properties in the second near-infrared (NIR-II) window. However, low quantum yield (QY) and poor uniformity of Ag2S QDs are still main obstacles for its application. In this work, a novel strategy of utilizing ultrasonic field is presented, which can enhance the microdroplet-based interfacial synthesis of Ag2S QDs. The ultrasound increases the presence of ions at the reaction sites by enhancing the ion mobility in the microchennels. Therefore, the QY is enhanced from 2.33 % (optimal QY without ultrasound) to 8.46 %, which is the highest value of Ag2S ever reported without ion-doping. Also, the decrease of the corresponding full width at half maximum (FWHM) from 312 nm to 144 nm indicates the obvious uniformity improvement of the obtained QDs. Further mechanism exploration illustrates that ultrasonic cavitation significantly increases the interfacial reaction sites by splitting the droplets. Meanwhile, the acoustic flow field strengthens the ion renewal at the droplet interface. Consequently, the mass transfer coefficient increases by more than 500 %, which is favorable to improve both the QY and quality of Ag2S QDs. This work serves both fundamental research and practical production for the synthesis of Ag2S QDs.

Inorganic-Organic Silica/PDMS Nanocomposite Antiadhesive Coating with Ultrahigh Hardness and Thermal Stability.

Antiadhesive surfaces have been gaining continuous attention, because of the scientific and industrial significance. Slippery surfaces and antismudge coatings with antiadhesive behavior have been readily designed and prepared. However, improving robustness of the surfaces, especially the simultaneous demonstration of features of high hardness, excellent adhesion to different substrates, and high thermal stability, is constantly challenging. Herein, we present a silica/polydimethylsiloxane (PDMS) nanocomposite coating (SPNC), wherein silica acts as a consecutive phase and nanophased PDMS is covalently embedded. The nanoconfined PDMS phase exhibits enhanced thermal stability and endows SPNC with slippery behavior; meanwhile, enrichment of PDMS on the surface renders a gradient composition of the coating. Accordingly, the inorganic-organic SPNC simultaneously displays a high nanoindentation hardness of 3.07 GPa and a pencil hardness over 9H, outstanding thermal stability of the slippery performance up to 400 °C, and excellent adhesion strength to different substrates. Additionally, SPNC exhibits high optical transparency, flexibility, resistance to bacterial clone, and chemical corrosion. With the scalable fabrication process, it can be envisioned that the antiadhesive coating with unprecedented comprehensive merits in this work has significant potentials for large-area applications, especially under severe service environments.

Ultrasonic assisted rapid preparation of superhydrophobic stainless steel surface and its application in oil/water separation.

The preparation of superhydrophobic (SH) surface on stainless steel by chemical etching method is challenging due to the good corrosion resistance of the material. In this work, SH surface with water contact angle (WCA) as high as 163.21° was accomplished on 304 stainless steel surface by a rapid ultrasonic-assisted chemical etching method within 7 min and a low-cost fluorine-free modification treatment. The mechanism of ultrasonic field on the etching process was explored by detecting the cavitation and oscillation energy in the reactor. It is the first time to found that the ultrasonic cavitation effect enhanced the etching process by both chemical and physical facilitation resulting in hierarchical lamellar micro-structures, "mountain-like" micro-structure clusters and "coral-reef-like" nano-scale structures on the surface. With the ultrasonic power increasing, the ultrasonic cavitation effect not only enhanced the superhydrophobicity of sample surface, but also improved the uniformity of surface wettability. The samples also showed excellent performance of oil/water separation for various organics (all separation efficiencies up to 96%) and remarkable mechanical stability.

Resistance Switching Behavior of a Perhydropolysilazane-Derived SiOx-Based Memristor.

SiOx is an important dielectric material layer for resistive switching memory due to its compatibility with complementary metal-oxide semiconductor (CMOS) technology. Here we propose a solution process for a SiOx dielectric layer based on perhydropolysilazane (PHPS). A series of SiOx layers with different compositions are prepared by controlling the conversion process from PHPS, then the resistance switching behaviors of typical Ag/SiOx/Au memristors are analyzed. The effect of oxygen vacancies and Si-OH groups on the formation and rupture of Ag conducting filaments (CFs) in the SiOx layer was thoroughly investigated. Ultimately, we achieved a high-performance memristor with a coefficient of variation (σ/µ) as low as 0.16 ± 0.08 and an on/off ratio as high as 106, which can rival the performance of the SiOx memristors based on the high-vacuum and high-cost vapor deposition methods. These findings demonstrate the high promise of the PHPS-derived SiOx dielectric layer in the field of memristors.

Flexible Hard Coatings with Self-Evolution Behavior in a Low Earth Orbit Environment.

Lightweight, long lifetime, and flexible polymer membrane-based structures, which are tightly folded on the ground and then unfolded in space, suffer from repeated bending before launching and fatal erosion on exposure to atomic oxygen (AO) in a low Earth orbit (LEO). Although various AO-resistant coatings have been developed, a coating that can simultaneously meet the critical requirements for the mechanical robustness and long-term protection of polymer membranes is rare. Here, we fabricated a coating with mechanical robustness and long-term space endurance, starting from an inorganic polymer precursor. A hybrid coating with a nanoscale polymer/silica bicontinuous phase is first prepared on the ground, which exhibits outstanding flexibility and excellent abrasion resistance. Then, the coating shows an in situ self-evolution behavior under AO and ultraviolet (UV) synergism to afford dense and crack-free silica coating with outstanding endurance. Our strategy displays great potential for protecting deployable membrane structures serving in the LEO.

Room-Temperature, Solution-Processed SiOx via Photochemistry Approach for Highly Flexible Resistive Switching Memory.

Due to its high versatility and cost-effectiveness, solution process has a remarkable advantage over physical or chemical vapor deposition (PVD/CVD) methods in developing flexible resistive random-access memory (RRAM) devices. However, the reported solution-processed binary oxides, the most promising active layer materials for their compatibility with silicon-based semiconductor technology, commonly require high-temperature annealing (>145 °C) and the RRAMs based on them encounter insufficient flexibility. In this work, an amorphous and uniform SiOx active layer was prepared by irradiating an inorganic polymer, perhydropolysilazane, with a vacuum ultraviolet of 172 nm at room temperature. The corresponding RRAM showed typical bipolar resistance switching with a forming-free behavior. The device on polyimide film exhibited outstanding flexibility with a minimum bending radius of 0.5 mm, and no performance degradation was observed after bending 2000 times with a radius of 2.3 mm, which is the best among the reported solution-processed binary oxide-based RRAMs and can even rival the performance of PVD/CVD-based devices. This room-temperature solution process and the afforded highly flexible RRAMs have vast prospects for application in smart wearable electronics.

Mechanism of ultrasonic impregnation on porosity of activated carbons in non-cavitation and cavitation regimes.

Ultrasonic impregnation has proven to be an effective method to improve surface area and pore volume during preparation of activated carbons. However, the mechanism by which the promotion effect of ultrasonic impregnation is still ambiguous. Fundamental wave pressure (FWP) and broadband integrated pressure (BIP) were used to estimate the non-cavitation (vibration) energy and cavitation energy, respectively. The effects of FWP and BIP on the pore volume, surface area, surface functional groups, and microcosmic morphology were investigated in non-cavitation and cavitation regimes. Ultrasonic vibration promoted the surface enlargement and pore development of activated carbons, and it mainly affected the development of mesopore volume (Vmes) in both the pore volume and the mesopore-size-distribution range. The Vmes was enhanced by 60%-100% in the non-cavitation regime. Ultrasonic cavitation also facilitated porosity development of activated carbons, and it mainly affected the development of specific surface area (SBET) and micropore volume (Vmic). The excessive cavitation led to a decrease of the porosity of activated carbons, so the BIP should be optimized during impregnation. The highest SBET, Vmic, and Vmes for activated carbons were obtained by in the presence of both FWP and BIP, which were enhanced by 29.05%, 30.23%, and 113.33%, respectively, compared with the corresponding value for the activated carbon prepared without using ultrasonic impregnation. This work provided new insight into the role of the acoustic energy present during impregnation in tuning properties of activated carbons.

Surfactant-free synthesis of hollow mesoporous carbon spheres and their encapsulated Au derivatives using biopolymeric chitosan.

To realize surfactant-free synthesis of biomass-derived hollow mesoporous carbon spheres and their derivatives, choice of synthetic methodology and carbon precursor is crucial. Herein, a brand-new hollow mesoporous carbon sphere (HMCS) is first synthesized from 8-quinolinol modified chitosan via an in situ stöber templating approach without surfactant followed by pyrolysis and alkali washing. The resultant HMCS is uniform, and shows a cavity size of 417 nm, a shell thickness of 5 nm, and a narrow mesopore size distribution centered at 3.9 nm. The HMCS is then upgraded by encapsulation of a single Au nanocrystal (NC) into the void of HMCS to form a yolk-shell architecture, YS-Au@HMCS. Its cavity size and shell thickness are decreased to 187 and 3 nm, while the mesopore size is increased to 4.3 nm, the surface area (215 m2 g-1) and mesoporosity (74.7%) are triple and twice that of HMCS, respectively, just by halving the delay time of carbon source addition. Owing to the unique hollow interiors and mesopores, as well as their synergism with the encapsulated Au NCs, the elaborately fabricated YS-Au@HMCS exhibits appealing catalytic performances towards the deposal of sewage. It delivers a large activity factor of 34.32, 13.29 and 0.05 s-1 g-1 in the reduction of 4-nitrophenol and methylene blue using sodium borohydride, and in the photodegradation of methylene blue under visible light irradiation, respectively. These advances shed new light on the synthesis of hollow mesoporous carbon spheres and the designed synthesis of functional carbon materials with versatile applications.

Influence of sound directions on acoustic field characteristics within a rectangle-shaped sonoreactor: Numerical simulation and experimental study.

Acoustic field intensity and distribution are the most important factors for the efficiency of ultrasonic processing. Recent simulation studies suggested that sound direction could influence both acoustic field intensity and distribution, but this influence has scarcely been investigated experimentally so far. In this work, we systematically studied the influence of sound directions on the acoustic field with up to five directions via both simulation and experiment. Fluid-structure interaction (FSI) harmonic response simulation and aluminum foil erosion experiment were employed to study the acoustic field under different directional combinations of ultrasonic sources. Results of simulation coincided well with that of experiment, which indicated that acoustic intensity, uniformity and cavitation characteristics were significantly affected by sound directions. Based on the results, several influence rules of sound directions were proposed. Optimal acoustic field with sound intensity of 30 times higher than that of single-wall excitation and severe cavitation volume of 95% was obtained. This work provides useful guidelines for acoustic field design of high-intensity ultrasonic apparatus.

Dense, uniform, smooth SiO2/TiO2 hard coatings derived from a single precursor source of tetra-n-butyl titanate modified perhydropolysilazane.

SiO2/TiO2 composite coatings are of great interest due to their optical, photocatalytic, electrical and mechanical properties. There are many methods for preparing SiO2/TiO2 composite coatings. Among these, the sol-gel process is eco-friendly and easily implementable for industrial applications. However, it is still a great challenge to prepare dense, uniform and smooth SiO2/TiO2 composite coatings with a sol-gel process. In this work, we show a modified sol-gel process for achieving dense, uniform and smooth SiO2/TiO2 coatings with tetra-n-butyl titanate modified perhydropolysilazane (PHPS) as a single precursor source, in which PHPS acts as the source for SiO2 instead of a traditional alkoxylsilane compound. The micro-morphology and composition evolution during the preparation process have been investigated; a smooth surface with a roughness average (S a) below 4.5 nm and a uniform distribution of Ti elements over the entire coating are shown. These dense, uniform SiO2/TiO2 coatings exhibit excellent mechanical robustness, with hardness values as high as 9.45 GPa, excellent optical transparency and hydrophilic properties.

Highly transparent and durable superhydrophobic hybrid nanoporous coatings fabricated from polysiloxane.

Highly transparent and durable superhydrophobic hybrid nanoporous coatings with different surface roughnesses were fabricated via a simple solidification-induced phase-separation method using a liquid polysiloxane (PSO) containing SiH and SiCH═CH2 groups as precursors and methyl-terminated poly(dimethylsiloxane)s (PDMS) as porogens. Owing to the existence of SiCHn units, the hybrid material is intrinsically hydrophobic without modification with expensive fluorinated reagents. The roughness of the coating can be easily controlled at the nanometer scale by changing the viscosity of PDMS to achieve both superhydrophobicity and high transparency. The influence of surface roughness on the transparency and hydrophobicity of the coatings was investigated. The enhancement from hydrophobic to superhydrophobic with increasing surface roughness can be explained by the transition from the Wenzel state to the Cassie state. The optimum performance coating has an average transmittance higher than 85% in the visible-light range (400-780 nm), a water contact angle of 155°, and a slide angle lower than 1°. The coatings also exhibit good thermal and mechanical stability and durable superhydrophobicity, which paves the way for real applications of highly transparent superhydrophobic coatings.

Thermal assisted ultrasonic bonding method for poly(methyl methacrylate) (PMMA) microfluidic devices.

A thermal assisted ultrasonic bonding method for poly(methyl methacrylate) (PMMA) microfluidic devices has been presented. The substrates were preheated to 20-30 degrees C lower than glass transition temperature (T(g)) of the polymer. Then low amplitude ultrasonic vibration was employed to generate facial heat at the interface of PMMA substrates. PMMA microfluidic chips were successfully bonded with bulk temperature well below T(g) of the material and with pressure two orders lower than conventional thermal bonding, which was of great benefit to reduce the deformation of microstructures. The bonding process was optimized by Taguchi method. This bonding technique showed numerous superiorities including high bonding strength (0.95MPa), low dimension loss (0.3-0.8%) and short bonding time. Finally, a micromixer was successfully bonded by this method and its performance was demonstrated.